液电脉冲低温等离子体催化氧化难降解有机废水的研究

In this project application, dyes wastewater (weak acid brilliant blue RAW, weak acid brilliant green GS) was selected as typical organic compounds for degradation by pulsed electrical discharge. A novel combined continuously-flow gas-liquid-solid hybrid discharge reactor was designed. The surface of the discharge electrodes were made by nanoporous-film consisted of catalysts. At the same time the porous solid adsorption/catalyst and Fenton reagents were added to the wastewater. The focus of the research was the cooperativity of the catalysts and Fenton reagents and the non-thermal plasmas. The kinetic model for wastewater degradation in hybrid discharge system was established from elementary reactions, herterogeneous transferring and chemical reactions. The various effects of contribution to the degradation were clarified and the reaction process was optimized by Matlab software. Through this project research, a deeper understanding of degradation of refractory organic wastewater by non-thermal plasma was achieved from the mechanism research. The gas-liquid-solid hybrid discharge simultaneously was realized by the preparation of the nanoporous-film electrodes. The porous solid adsorption/catalyst and Fenton reagents were integrated into the system. A novel combined continuously-flow gas-liquid-solid hybrid discharge reactor was developed. This project research was provided to the applications of this technology for industrialization.

以蒽醌类染料废水（弱酸艳蓝RAW，弱酸艳绿GS）为目标污染物和研究对象，建立一套新型气-液-固三相同时放电的组合式连续流反应器，将放电极板表面制成由催化剂组成的纳米多孔膜，同时在液相中加入多孔固体吸附/催化剂和芬顿试剂，重点研究纳米电极、多孔固体吸附/催化剂和芬顿反应联合作用的化学过程与非平衡等离子体之间的协同效应；从基元反应出发结合多相传递过程和化学反应过程的分析，建立气-液-固三相放电等离子体反应器降解有机污染物的数学模型；并阐明各种效应对降解过程的贡献，应用Matlab软件进行反应过程的最优化。通过本项目的研究，从机理上对非平衡等离子体降解有毒有害有机废水进行更深入的理解，并形成定量化的描述；在技术上通过制备纳米多孔膜电极实现气-液-固三相同时放电，并引入固体吸附/催化剂和芬顿试剂，开发出新型组合式连续流反应器，为非平衡等离子体催化氧化有毒有害废水的工业化应用提供技术准备和支持。

研究蒽醌类染料废水处理技术对印染行业的良性发展具有积极意义，本研究项目通过研制筛选高效纳米多孔膜光电催化剂电极，实现纳米孔形状和孔径的准确调控。同时，利用纳米多孔膜光电催化剂电极协同高压脉冲放电等离子体催化氧化蒽醌类染料废水，采用Box-Behnken响应面优化实验设计，并对实验结果用软件Design-Experts 8.0进行方差分析。在pH为6.88，脉冲峰值电压为23kV，脉冲频率为300Hz，电极距离为1cm，反应30min，弱酸艳绿GS废水的色度去除率可达99.89%。利用UV-Vis、FTIR和GC-MS等对高压脉冲放电等离子体体系中弱酸艳绿GS、弱酸艳蓝RAW、活性黄X-RG和直接耐酸大红4BS在反应过程中的中间产物及反应路径进行了详细的研究, 为液电脉冲低温等离子体催化氧化有毒有害废水的工业化应用提供了技术准备和支持。